Abstract

Abstract. A full diurnal measurement of stratospheric column NO2 has been made over the Jet Propulsion Laboratory's Table Mountain Facility (TMF) located in the mountains above Los Angeles, California, USA (2.286 km above mean sea level, 34.38∘ N, 117.68∘ W). During a representative week in October 2018, a grating spectrometer measured the telluric NO2 absorptions in direct solar and lunar spectra. The stratospheric column NO2 is retrieved using a modified minimum-amount Langley extrapolation, which enables us to accurately treat the non-constant NO2 diurnal cycle abundance and the effects of tropospheric pollution near the measurement site. The measured 24 h cycle of stratospheric column NO2 on clean days agrees with a 1-D photochemical model calculation, including the monotonic changes during daytime and nighttime due to the exchange with the N2O5 reservoir and the abrupt changes at sunrise and sunset due to the activation or deactivation of the NO2 photodissociation. The observed daytime NO2 increasing rate is (1.34±0.24)×1014 cm−2 h−1. The observed NO2 in one of the afternoons during the measurement period was much higher than the model simulation, implying the influence of urban pollution from nearby counties. A 24 h back-trajectory analysis shows that the wind first came from inland in the northeast and reached southern Los Angeles before it turned northeast and finally arrived at TMF, allowing it to pick up pollutants from Riverside County, Orange County, and downtown Los Angeles.

Highlights

  • Nitrogen dioxide (NO2) plays a dominant role in the ozone (O3)-destroying catalytic cycle (Crutzen, 1970)

  • The ambient twilight in the background of the moonlight occultation should be accounted for in the NO2 retrieval, which is beyond the scope of this work

  • We have presented the diurnal measurements of stratospheric column NO2 that have been made over the Table Mountain Facility (TMF) located in Wrightwood, California (2.286 km, 34.38◦ N, 117.68◦ W), from 23 to 28 October 2018

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Summary

Introduction

Nitrogen dioxide (NO2) plays a dominant role in the ozone (O3)-destroying catalytic cycle (Crutzen, 1970). Since the optical path of sun/moonlight at dawn or dusk (solar/lunar zenith angle ≈ 90◦) is much longer than the optical path of the direct sunlight at noon–midnight, the NO2 absorption in the noon–midnight spectrum can be assumed to be small, and the NO2 absorption in the twilight slant column could be isolated effectively by ratioing the scattered twilight spectrum to the scattered noon spectrum. This DOAS principle applies to ratios of direct moonlight or sunlight at low and high air mass factors. The effect of urban pollution on the measured NO2 can be deduced from this comparison

Instrumentation and measurement technique
The DOAS retrieval
The photochemical model
Diurnal variation in stratospheric column NO2
Vertical profile of NO2 production and loss
Daytime NO2 increasing rate
Temperature sensitivity
Back-trajectories
Summary
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